First-Principles Study of C-C Coupling Pathways for CO2Electrochemical Reduction Catalyzed by Cu(110)

Tung Chun Kuo, Jia Wei Chou, Min Hsiu Shen, Zih Siang Hong, Tzu Hsuan Chao, Qi Lu, Mu Jeng Cheng

Research output: Contribution to journalArticlepeer-review

Abstract

To build a carbon-neutral energy cycle, the development of electrocatalysts that can reduce CO2 into products containing at least two carbon atoms (C2+) is crucial. This process would require at least one C-C coupling of two C1 intermediates. The (110) facet of copper is known for its ability to reduce CO2 to C2+ products in high quantities (Faradaic efficiency ≥65%). In this study, we used constant electrode potential density functional theory calculations to determine the dominant C-C coupling pathways for CO2 electrochemical reduction (CO2ER) on Cu(110). By studying the mechanism of CO2ER to methane, we identified *CO and *CH as high-concentration C1 species due to their high ΔG‡ for further hydrogenation. Based on this result, 26 C-C coupling reactions that contain at least one high-concentration C1 intermediate were selected for investigation. The most important ones responsible for C2+ formation on Cu(110) were identified, and the influence of strain on the rates of these reactions was also investigated.

Original languageEnglish
Pages (from-to)2464-2476
Number of pages13
JournalJournal of Physical Chemistry C
Volume125
Issue number4
DOIs
Publication statusPublished - 2021 Feb 4

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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